High temperature superconductors (HTS) have been driving research and development programs for about three decades now and are on the verge of entering large scale utilization in the form of Coated Conductors (CCs), a robust and flexible tape architecture that enables textured growth of the rather brittle material class. A remaining bottleneck for widespread CC implementation is the high cost/performance ratio, essentially controlled by the complex and decelerating step of HTS layer growth. In this thesis we challenge the throughput and cost constraints of conventional growth methods through development of a novel growth technique that combines Chemical Solution Deposition (CSD), an inherently low-cost precursor deposition approach, with a high growth rate, non-equilibrium growth scheme that allows the formation of a transient (Ba-Cu-O) liquid phase prior to crystallization of the final product phase: Transient Liquid-Assisted Growth via CSD (TLAG-CSD).
We employed the new process to grow YBa2Cu3O7-d (YBCO) thin films, a cuprate-based HTS material with unmatched current carrying performance in applied magnetic field conditions and at high temperatures. The unprecedented properties can only be reached if the electrically anisotropic compound exhibits biaxial texture and provides sufficient nanometric defects to pin vortices. Hence, not only is the fundamental understanding of the TLAG-CSD process required but also ways to promote epitaxial growth at high rates, avoidance of any current-degrading sources and strategies to enrich the pinning landscape. To tackle these challenges, we combined several advanced characterization methods: In-situ growth experiments at a synchrotron facility were carried out to follow growth kinetics under variation of total and oxygen partial pressures, growth temperatures, heating ramps, film thickness/composition and nanoparticle (NP) addition. The combined set of experiments was successfully summarized in the form of so-called kinetic phase diagrams, a visual representation of the out-of-equilibrium processes and a roadmap for its utilization.
Epitaxial, c-axis oriented YBCO films were thoroughly studied via X-ray diffraction, transmission electron microscopy (TEM), low temperature electrical transport and inductive measurements to identify process related limitations and opportunities. This includes probing of the YBCO microstructuture and intrinsic electrical properties to avoid liquid induced substrate reactivity, segregation of secondary phases, while enabling proper CO2 elimination and oxygen doping of the crystal structure.
We disclose that epitaxial layer growth rates above 100nm/s can be accomplished through the TLAG-CSD approach, surpassing conventional techniques used in CC manufacturing schemes (TFA-CSD/PLD/MOCVD) by up to two orders of magnitude. Superconducting films are demonstrated to reach high epitaxial grain alignment (Δω<0.6º and Δφ<1º), optimal critical temperatures (Tc=88-92K) and competitive critical current densities (Jc(77K)=2-5MA/cm2). We further classify the TLAG-CSD process as highly versatile in enriching the vortex pinning landscape, not only through its capability to promote a high density of stacking faults and small ab-oriented YBCO grains (5-10nm) in pristine YBCO films, but also through its compatibility with preformed nanoparticle addition in nanocomposites.
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